We present and overview of research conducted at the National Institute of Standards and Technology aimed at developing combinatorial and high throughput measurement approaches to polymer surfaces, interfaces and thin films. Topics include, 1) the generation of continuous gradient techniques for fabricating combinatorial libraries of film thickness, temperature, surface chemistry and polymer blend composition; 2) high-throughput measurement techniques for assessing the mechanical properties and adhesion of surfaces, interfaces and films; and 3) microfluidic approaches to synthesizing and analyzing libraries of interfacially active polymer species.